Arsenic (As) contaminated groundwater is a worldwide concern due to its chronic effects on human health. The objectives of the study were to evaluate natural inexpensive raw laterite (RL) and kaolinite (RK) for their potential use as As sorbents and to understand the As sorption on laterite and kaolinite by employing sorption and kinetic models. Raw laterite and RK were tested for EC, pH, XRF and CEC as basic parameters. Batch sorption and kinetic experiments data were fitted in the sorption (Langmuir and Freundlich) model and kinetic (pseudo-first and pseudo-second order) reaction equations, respectively. Morphological and structural changes were observed in RL and RK samples before and after As saturation by employing FTIR and SEM. The major constituent in RL was Fe and Al oxides while in RK major oxides were silica and Al. The Freundlich sorption model well explained the experimental data, indicating a greater sorption capacity of RL on a hetero-layered surface compared to RK. The kinetic reaction equations showed that equilibrium was achieved after a contact time of 240 min and the adsorption was chemisorption in nature. The RL and RK were found to be effective sorbents for As removal, however, RL showed maximum As adsorption and thus superior in comparison with RK. Structural and morphological characterization reveals the role of Fe and Al oxides in the case of RL, and Al oxides in the case of RK, in the adsorption of As. Hence this study concludes that these naturally occurring inexpensive resources can be used as sorbent agents for As-contaminated drinking water treatment.